WO2006123892A9 - Lieur de polymere destine a un dispositif electrochimique comprenant plusieurs piles electrochimiques empilees - Google Patents

Lieur de polymere destine a un dispositif electrochimique comprenant plusieurs piles electrochimiques empilees Download PDF

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Publication number
WO2006123892A9
WO2006123892A9 PCT/KR2006/001838 KR2006001838W WO2006123892A9 WO 2006123892 A9 WO2006123892 A9 WO 2006123892A9 KR 2006001838 W KR2006001838 W KR 2006001838W WO 2006123892 A9 WO2006123892 A9 WO 2006123892A9
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Prior art keywords
binder
electrochemical device
separator
electrode
active material
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PCT/KR2006/001838
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English (en)
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WO2006123892A1 (fr
Inventor
Byoung-Yun Kim
Dong-Jo Ryu
Ju-Hyun Kim
Chang-Sun Han
Eun-Young Goh
Hyang-Mok Lee
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Lg Chemical Ltd
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Priority to JP2008511060A priority Critical patent/JP5110599B2/ja
Publication of WO2006123892A1 publication Critical patent/WO2006123892A1/fr
Publication of WO2006123892A9 publication Critical patent/WO2006123892A9/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
    • C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
    • C08F220/10—Esters
    • C08F220/12—Esters of monohydric alcohols or phenols
    • C08F220/16—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms
    • C08F220/18—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms with acrylic or methacrylic acids
    • C08F220/1804—C4-(meth)acrylate, e.g. butyl (meth)acrylate, isobutyl (meth)acrylate or tert-butyl (meth)acrylate
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
    • C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
    • C08F220/10—Esters
    • C08F220/12—Esters of monohydric alcohols or phenols
    • C08F220/16—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms
    • C08F220/18—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms with acrylic or methacrylic acids
    • C08F220/1808—C8-(meth)acrylate, e.g. isooctyl (meth)acrylate or 2-ethylhexyl (meth)acrylate
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/04—Construction or manufacture in general
    • H01M10/0413—Large-sized flat cells or batteries for motive or stationary systems with plate-like electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F212/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring
    • C08F212/02—Monomers containing only one unsaturated aliphatic radical
    • C08F212/04—Monomers containing only one unsaturated aliphatic radical containing one ring
    • C08F212/06—Hydrocarbons
    • C08F212/08—Styrene
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
    • C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
    • C08F220/10—Esters
    • C08F220/12—Esters of monohydric alcohols or phenols
    • C08F220/16—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms
    • C08F220/18—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms with acrylic or methacrylic acids
    • C08F220/1802—C2-(meth)acrylate, e.g. ethyl (meth)acrylate
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F222/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a carboxyl radical and containing at least one other carboxyl radical in the molecule; Salts, anhydrides, esters, amides, imides, or nitriles thereof
    • C08F222/04—Anhydrides, e.g. cyclic anhydrides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0085—Immobilising or gelification of electrolyte
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a binder, which has excellent adhesion and thermal bonding characteristics and is useful for a high-capacity electrochemical device comprising multiply stacked electrochemical cells, an electrode comprising the same binder, and an electrochemical device, preferably a lithium secondary battery, having improved overall quality by using the same electrode.
  • lithium secondary batteries developed in early 1990's, have a drive voltage and an energy density higher than those of conventional batteries using aqueous electrolytes (such as Ni-MH batteries, Ni-Cd batteries and H 2 SO 4 -Pb batteries), and thus are spotlighted in the field of secondary batteries.
  • aqueous electrolytes such as Ni-MH batteries, Ni-Cd batteries and H 2 SO 4 -Pb batteries
  • lithium secondary batteries have a problem related to their safety, due to ignition and explosion caused by the use of an organic electrolyte.
  • lithium secondary batteries have a disadvantage in that they are manufactured via a relatively complicated manufacturing process.
  • a lithium ion polymer battery developed recently, can improve the aforementioned problem and disadvantage of a lithium ion battery, and thus has been regarded as one of the most potent candidates for next- generation batteries.
  • a lithium ion polymer battery shows a relatively lower capacity as compared to a lithium ion battery, and has an insufficient discharge capacity, particularly at low temperature.
  • the capacity of a battery is in proportion to the content of an electrode active material, it is very important to design a cell structure in such a manner that as much an electrode active material as possible can be packed in a limited space provided by a battery pack.
  • 2001-0082058 and 2001-0082059 disclose an electrochemical device, which is manu- factured with ease and has an efficient space structure sufficient to maximize the amount of an electrode active material, the electrochemical device comprising multiply stacked electrochemical cells.
  • the basic unit of the stacked electrochemical cells is a full cell or a bicell.
  • Characteristics of a full cell or a bicell largely depend on the electrode, electrolyte and other materials used therein. Particularly, because the content of the active material introduced into an electrode is ultimately related to the maximum amount of lithium ions capable of binding, the capacity of a battery is in proportion to the content of an electrode active material. Hence, if a binder having excellent adhesion so as to reduce the amount of a binder, it is possible to provide an electrode comprising an active material in an amount increased accordingly. Therefore, there has been a need for a novel binder having excellent adhesion.
  • PVDF-based polymers include PVDF homopolymer, and PVDF copolymers such as polyvinylidene fluoride- hexafluoropropylene copolymer (Korean Laid-Open Patent No. 2001-0055968) and polyvinylidene fluoride-chlorotrifluoroethylene copolymer.
  • PVDF-based polymers are advantageous in that they are chemically and electrochemically stable.
  • the present invention has been made in view of the above-mentioned problems.
  • the inventors of the present invention have prepared binders by polymerizing copolymerizable monomers, forming a binder, with various compositional ratios.
  • the inventors have found a binder composition, which uses water as a dispersion medium, and thus is environmentally-friendly, imparts sufficient adhesion between a collector and an active material even when used in a small amount to provide a battery with high-capacity, and maintains adhesion after thermal bonding to provide excellent thermal bonding characteristics between an electrode and a separator, so as to be used in a high-capacity electrochemical device comprising multiply stacked electrochemical cells.
  • the present invention is based on this finding.
  • the present invention is characterized by providing an environmentally-friendly binder, suitable for the production of a novel electrochemical device, which is manufactured via a simple process compared to a conventional process for manufacturing cells, and utilizes its inner space more efficiently so as to obtain high capacity.
  • an environmentally-friendly binder suitable for the production of a novel electrochemical device, which is manufactured via a simple process compared to a conventional process for manufacturing cells, and utilizes its inner space more efficiently so as to obtain high capacity.
  • a plurality of full cells or bicells are stacked by using each full cell or bicell as a basic unit cell, a separator is inserted into each overlapped portion in the full cells or bicells, and then the separator is bonded thereto by way of hot fusion (see FIGs. 2 and 3).
  • the binder contains a maximized amount of monomer capable of controlling adhesion property while ensuring its physical stability. Hence, the binder can maintain the adhesion between an electrode and a separator continuously even during and after carrying out hot fusion. Accordingly, it is possible to improve the structural stability of an electrode and multiply stacked electrochemical cells comprising the electrode, thereby improving the lifespan characteristics of the device. At the same time, it is possible to improve the rate characteristics of a battery through the activation of electrode reactions, caused by the efficient space structure of the electrochemical device in which a plurality of unit cells are stacked so as to realize high capacity.
  • the first monomer (a), forming the binder polymer according to the present invention is a conventional monomer that is known to one skilled in the art as a monomer capable of controlling the quality of a battery.
  • a (meth)acrylic acid ester monomer which improves rate characteristics of a battery by increasing the affinity to an electrolyte and shows excellent adhesion to a collector, may be used as the first monomer.
  • Non-limiting examples of such (meth)acrylic acid ester monomers include: (1) acrylate monomers (e.g., methyl acrylate, ethyl acrylate, propyl acrylate, isopropyl acrylate, n-butyl acrylate, isobutyl acrylate, n-amyl acrylate, isoamyl acrylate, n-hexyl acrylate, 2-ethylhexyl acrylate, hydroxyethyl acrylate, hydroxypropyl acrylate, lauryl acrylate); (2) methacrylate monomers (e.g., methyl methacrylate, ethyl methacrylate, propyl methacrylate, isopropyl methacrylate, n-butyl methacrylate, isobutyl methacrylate, n-amyl methacrylate, isoamyl methacrylate, n-hexyl methacrylate,
  • the (meth)acrylic acid ester monomer is used preferably in an amount of 20-79 parts by weight per 100 parts by weight of the binder polymer according to the present invention. If the (meth)acrylic acid ester monomer is used in an amount of less than 20 parts by weight, adhesion characteristics of the binder may be degraded significantly. If the (meth)acrylic acid ester monomer is used in an amount of greater than 79 parts by weight, it may not be possible to prepare the binder itself because of low stability of the binder during the preparation thereof.
  • the vinyl monomer is used preferably in an amount of 20-60 parts by weight per 100 parts by weight of the binder polymer, but is not limited thereto. If the vinyl monomer is used in an amount of less than 20 parts by weight, it may not be possible to prepare the binder itself because of low stability of the binder during the preparation thereof. If the vinyl monomer is used in an amount of greater than 60 parts by weight, the binder shows a significantly decreased adhesion value because such a large amount of vinyl monomer increases the glass transition temperature.
  • unsaturated monocarboxylic acid monomers e.g., acrylic acid, methacrylic acid, etc.
  • unsaturated dicarboxylic acid monomers e.g., itaconic acid, fumaric acid, citraconic acid, methaconic acid, glutaconic acid, crotonic acid, isocrotonic acid, etc.
  • acrylamide monomers e.g., acrylamide, n-methylolamide, n- butoxymethylacrylamide, etc
  • methacrylamide monomers e.g., methacrylamide, n-methylol methacrylamide, n-butoxymethylmethacrylamide, etc.
  • the binder according to the present invention that satisfies the aforementioned conditions shows excellent properties, including adhesion in an electrode and adhesion between an electrode and a collector, and thermal bonding characteristics between an electrode and a separator, and provides a battery with excellent characteristics such as rate characteristics and lifespan characteristics, as compared to a binder according to the prior art.
  • the aforementioned monomers except the unsaturated carboxylic acid monomer (c) i.e., the acrylate (methacrylate) monomer (a) and the vinyl monomer (b)
  • the aforementioned monomers except the unsaturated carboxylic acid monomer (c) can control the overall quality of a battery, including initial capacity, initial efficiency, capacity variation during repeated charge/discharge cycles or other physical properties of a battery.
  • the present invention it is also possible to maximize the adhesion value between an electrode and a collector and the thermal bonding effect between an electrode and a collector via hot fusion by using the monomer capable of controlling the adhesion (such as an unsaturated carboxylic acid monomer), to the maximum extent.
  • the monomer capable of controlling the adhesion such as an unsaturated carboxylic acid monomer
  • the above effects can be obtained from the chemical bond, such as the ionic bond, formed between the carboxyl (-C00H) group present in the unsaturated carboxylic acid monomer and copper ions contained in a copper collector.
  • the molecular weight modifier that may be used in the present invention includes t- dodecyl mercaptan, n-dodecyl mercaptan, n-octyl mercaptan, or the like.
  • any compound that causes generation of radicals may be used, and particular examples thereof include ammonium persulfate, potassium persulfate, sodium persulfate, benzoyl peroxide, butyl hydroperoxide, cumene hydroperoxide, azobisisobutyronitrile, or a mixture thereof.
  • a water soluble or redox polymerization initiator is preferred.
  • the polymer particles according to the present invention may be prepared by a conventional polymerization process known to one skilled in the art, for example, by an emulsion polymerization process, a suspension polymerization process, a dispersion polymerization process, a two-step polymerization process using seed polymerization, or the like.
  • polymerization temperature and polymerization time may be selected depending on the kind of the polymerization initiator used for the poly- merization. For example, polymerization may be carried out at a temperature of about 30- 100 0 C for 0.5-20 hours.
  • solvent or the dispersion medium used for the binder composition according to the present invention there is no particular limitation in the solvent or the dispersion medium used for the binder composition according to the present invention. However, it is preferable to use a solvent or a dispersion medium present in a liquid state at room temperature under ambient pressure, because such solvents or dispersion media allow the polymer particles to maintain the shape, when electrode slurry comprising the binder composition is applied onto a collector and then dried.
  • the dispersion medium that may be used in the present invention is one capable of dispersing the polymer particles and an electrode active material.
  • the dispersion medium include water; alcohols such as methanol, ethanol, propanol, isopropanol, butanol, isobutanol, s-butanol, t-butanol, pentanol, isopentanol, hexanol, or the like; ketones such as acetone, methyl ethyl ketone, methyl propyl ketone, ethyl propyl ketone, cyclopentanone, cyclohexanone, cycloheptanone, or the like; ethers such as methyl ethyl ether, diethyl ether, dipropyl ether, diisopropyl ether, dibutyl ether, diisobutyl ether, di n-amyl ether, di
  • the present invention provides slurry for an electrode, which comprises: (a) the binder as defined above; and (b) an electrode active material. If desired, the slurry may further comprise other additives generally known to one skilled in the art.
  • the electrode active material is the most important material that determines the capacity of a battery.
  • Any cathode active material generally used in a lithium secondary battery can be used in the present invention, and non-limiting examples of such cathode active materials include metal oxides such as lithiated cobalt oxides, lithiated nickel oxides, lithiated manganese oxides, etc., or composite oxides formed by combination thereof, conductive polymers such as polypyrole, polyaniline, poly- acetylene, polythiophene, etc., or composite oxides formed by combination of a metal oxide with a conductive polymer.
  • the electrode slurry may further comprise a conductive agent, a viscosity modifier, a supplementary binder, or the like, in addition to the aforementioned active material.
  • viscosity modifier examples include water soluble polymers such as carboxymethyl cellulose, car- boxyethyl cellulose, ethyl cellulose, hydroxymethyl cellulose, hydroxypropyl cellulose, carboxyethylmethyl cellulose, polyethylene oxide, ethylene glycol, or the like, but are not limited thereto.
  • the present invention also provides an electrode for an electrochemical device, preferably for a lithium secondary battery, which comprises the slurry comprising the binder according to the present invention and an electrode active material.
  • the electrode may be manufactured by a method generally known to one skilled in the art.
  • electrode slurry comprising a mixture of the binder composition with an active material is applied onto a current collector, and the dispersion medium is removed by drying or by other means, so that the active material particles are bonded to the current collector and are bonded among themselves.
  • the present invention also provides an electrochemical device comprising the multiply stacked electrochemical cells using the binder.
  • the electrochemical device according to the present invention is an electrochemical device having such a structure that the content of an electrode active material can be maximized by utilizing the space of the electrochemical device with a significantly higher efficiency compared to a conventional electrochemical device.
  • a plurality of full cells or bicells are stacked as basic unit cells, and a separator is inserted into each overlapped portion in the full cells or bicells by way of thermal bonding using hot fusion technique (see FIGs. 2 and 3).
  • the full cell means an electrochemical cell comprising a cathode, a separator or an anode, in order or inverse order.
  • the bicell means an electrochemical cell including an electrode having one polarity at the center thereof and electrodes having the opposite polarity at both sides thereof.
  • the bicell comprises: a cathode, a separator, an anode, a separator, and a cathode; or an anode, a separator, a cathode, a separator, and an anode.
  • each full cell or bicell present at the outermost part of the electrochemical device includes an electrode comprising an electrode active material coated on the surface of a collector, such as a cathode comprising a cathode collector whose surface is coated with a cathode active material, or an anode comprising an anode collector whose surface is coated with an anode active material.
  • collector foil may be used instead of the single-side coated active material layer (see FIGs. 2 and 3).
  • both surfaces of a current collector may be coated with the same electrode active material.
  • the active material present on the outer surface which is not utilized in a unit cell, can form another full cell along with an active material coated on the counter electrode of another unit cell, adjacent to the unit cell. Therefore, as shown in FIG. 1, it is possible to solve the problems occurring when a single surface of a current collector is coated with an electrode active material, such problems being that the number of electrodes increases and the efficiency of a battery decreases as determined in terms of the space and weight of a battery. It is also possible to improve the overall quality of a battery by activating reactions in the battery by virtue of the efficient space structure of the electrochemical device.
  • the electrochemical device according to the present invention includes any device in which electrochemical reactions are performed. Particular examples thereof include all types of primary batteries, secondary batteries, fuel cells, solar cells, super capacitors, ultra capacitors and pseudo capacitors, and various sensors, electrolyzing devices and electrochemical reactors.
  • the electrochemical device according to the present invention is a secondary battery, including a lithium metal secondary battery, a lithium ion secondary battery, a lithium polymer secondary battery, or a lithium ion polymer secondary battery.
  • the electrochemical device is a lithium ion polymer battery.
  • the electrochemical device according to the present invention may be manufactured by a conventional method known to one skilled in the art.
  • a preferred embodiment of the method comprises the steps of: (a) providing a first outermost full cell, a second outermost full cell and an inner full cell interposed between both full cells; (b) stacking the first outermost full cell, the inner full cell and the second outermost full cell, in turn, in such a manner that the collector of each single-side coated electrode is located at the outermost layer, inserting a separator into each overlapped portion of the full cells, and bonding the separator to the full cells via hot fusion to provide a stacked structure; and (c) introducing the stacked full cells into a battery casing, injecting an electrolyte thereto, and sealing the battery casing.
  • a bicell for example, cathode-separator-anode-separator-cathode, or anode- separator-cathode-separator-anode, may be manufactured by stacking a separator on one electrode of both electrodes of the full cell obtained from step (iii) and further stacking the counter electrode thereon.
  • the electrolyte that may be used in the present invention includes a salt represented by the formula of A + B-, wherein A + represents an alkali metal cation selected from the group consisting of Li + , Na + , K + and combinations thereof, and B- represents an anion selected from the group consisting of PF 6 " , BF 4 -, Q-, Br, I , ClO 4 -, AsF 6 " , CH 3 CO 3 -, N(CF 3 SO 2 V, C(CF 2 SO 2 V and combinations thereof, the salt being dissolved or dissociated in an organic solvent selected from the group consisting of propylene carbonate (PC), ethylene carbonate (EC), diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), ethyl methyl carbonate (EMC), dimethyl sulfoxide, acetonitrile, dimethoxyethane, diethoxyethane, tetrahydrofuran, N- methyl
  • the separator is a porous substrate having pores.
  • the separator allows adhesion to an electrode via hot fusion.
  • there is no particular limitation in the temperature and pressure for such hot fusion as long as the separator can be adhered to the electrode.
  • hot fusion may be performed at a temperature of 60- 100 0 C and a pressure of 1-5 kgf.
  • the separator may be provided in the form of a membrane, a film or fiber.
  • the gelled polymer there is no particular limitation in the gelled polymer, as long as the polymer can be gelled upon swelling with an electrolyte.
  • the separator having a gelled polymer coating layer formed thereon may be fabricated by a conventional method known to one skilled in the art. In one embodiment of the method, a gelled polymer, for example PVdF copolymer is dissolved in a solvent, and the resultant solution is coated onto a separator, followed by drying.
  • the electrochemical device is a prismatic battery.
  • a casing for packing an electrochemical device is an aluminum prismatic can or aluminum laminate film. Because the structure of the electrochemical device according to the present invention has the same shape as a prismatic casing, there is no vacancy inside of the casing after inserting the electrochemical device into the casing. Therefore, it is possible to realize a highly integrated device, preferably a highly integrated battery, which permits active materials to utilize the space to the highest degree, resulting in a significant increase in the bulk energy density of a battery.
  • FIG. 3 is a schematic view showing the layered structure of stacked cells including bicells (a first outer bicell and a second outer bicell), each comprising partially single side-coated electrodes and a separator, and a bicell (inner bicell) comprising double side-coated electrodes and a separator; and [67] FIGs. 4-6 are photographic views showing the thermal bonding characteristics of multiply stacked cells using the binders according to Example 1 (FIG. 4), Example 2
  • a reaction mixture obtained by mixing and emulsifying 93.Og of ion exchange water, 30.0g of styrene, 60. Ig of butyl acrylate, 0.8g of aryl methacrylate, 4.4g of itaconic acid, 6g of acrylic acid and 0.15g of sodium lauryl sulfate was introduced in portions over 3 hours, while 0.21g of potassium persulfate dissolved in 10.0g of ion exchange water was also introduced in portions over 3 hours to provide a binder polymer.
  • a binder composition for an anode was obtained by adding potassium hydroxide to the binder polymer to adjust the pH to 7. The binder composition was used to manufacture an anode.
  • the polymerized binder was determined for the physical properties by measuring the final particle diameter, glass transition temperature and gel content. After measuring the particle diameter by using a light scattering device, the binder polymer had a particle diameter of 195 nm. After measuring the glass transition temperature by using a DSC (differential scanning calorimeter) under a heating rate of 10°C/min., the binder polymer had a glass transition temperature of -5°C. Additionally, the binder polymer had a gel content of 85% after the measurement using toluene as a solvent.
  • LiCoO 2 , carbon black and PVdF were dispersed in NMP in a weight ratio of LiCoO 2 : carbon black: PVdF of 95:2.5:2.5 to form slurry. Then, the slurry was coated onto aluminum foil, and dried at 130 0 C sufficiently, followed by pressing to provide a cathode.
  • the anode to be used as an anode disposed at the outermost layer of the outermost full cell was coated with slurry on one surface of the copper foil, thereby providing an anode comprising a copper anode collector coated with an anode active material on one surface thereof.
  • the anode to be used as an anode disposed at the inner part of the full cell was coated with slurry on both surfaces of the copper foil, thereby providing an anode comprising a copper anode collector coated with an anode active material on both surfaces thereof.
  • the single-side coated anode and the double-side coated anode had a thickness of 100/M and 135/M, respectively.
  • a polypropylene film having a microporous structure and a thickness of 16/M was used as a first polymer separator. Then, a multilayer polymer film was manufactured by using polyvinylidnene fluoride-chlorotrifluoroethylene copolymer 32008 available from Solvey Polymer Company as a second gelled polymer. In other words, 6g of the copolymer 32008 was introduced into 194g of acetone and stirred thoroughly while maintaining the temperature at 5O 0 C. After 1 hour, transparent solution, in which the copolymer 32008 was dissolved completely, was coated onto the first polymer separator via a coating process. The copolymer 32008 was coated to a thickness of 1/M, and the finally formed multilayer polymer film had a thickness of 18/M.
  • the cathode comprising a cathode collector coated with a cathode active material on both surfaces thereof was cut into a rectangular shape having a size of 2.9cm X 4.3cm with the exception of a portion corresponding to a tab.
  • the anode comprising an anode collector coated with an anode active material on both surfaces thereof was cut into a rectangular shape having a size of 3.0cm X 4.4cm with the exception of a portion corresponding to a tab.
  • the multilayer polymer film obtained as described above was cut into a size of 3.1cm X 4.5cm and was inserted between the cathode and the anode to provide an electrode assembly. Then, the electrode assembly was passed through a roll laminator at 100 0 C to perform thermal bonding between each electrode and the separator, thereby providing an inner full cell.
  • the cathode comprising a cathode collector coated with a cathode active material on one surface thereof was cut into a rectangular shape having a size of 2.9cm X 4.3cm with the exception of a portion corresponding to a tab.
  • the anode comprising an anode collector coated with an anode active material on both surfaces thereof was cut into a rectangular shape having a size of 3.0cm X 4.4cm with the exception of a portion corresponding to a tab.
  • the multilayer polymer film obtained as described above was cut into a size of 3.1cm X 4.5cm and was inserted between the cathode and the anode to provide an electrode assembly. Then, the electrode assembly was passed through a roll laminator at 100 0 C to perform thermal bonding between each electrode and the separator, thereby providing a first outermost full cell.
  • the cathode comprising a cathode collector coated with a cathode active material on both surfaces thereof was cut into a rectangular shape having a size of 2.9cm X 4.3cm with the exception of a portion corresponding to a tab.
  • the anode comprising an anode collector coated with an anode active material on both surfaces thereof was cut into a rectangular shape having a size of 3.0cm X 4.4cm with the exception of a portion corresponding to a tab.
  • Example 1 Seed (1) obtained from Example 1 was used and the monomers for emulsion polymerization, which had various compositions as described in the following Table 2, were introduced thereto to provide binder polymers, in the same manner as described in Example 1.
  • the physical properties of the binder polymers were also shown in Table 2.
  • the binder polymers according to Examples 8-10 had a different glass transition temperature
  • the binder polymers according to Examples 11-13 has a different gel content
  • the binder polymers according to Examples 14 and 15 had a different particle size.
  • the seed used to provide the binder polymers according to Examples 14 and 15 was obtained by using sodium lauryl sulfate in an amount of 0.3g and 0.06g, respectively.

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Abstract

L’invention concerne un dispositif électrochimique comprenant : (A) un lieur comprenant des particules polymères obtenues par la polymérisation de : (a) 20 à 70 parts en poids d’un monomère d’ester d’acide (méth)acrylique ; (b) 20 à 60 parts en poids d’un monomère vinylique ; et (c) 0,01 à 30 parts en poids d’un monomère d’acide carboxylique non saturé, basé sur 100 parts en poids d’un polymère lieur ; et (B) des piles électrochimiques empilées en utilisant ledit lieur, où ledit lieur permet aux particules de matériau actif d’électrodes d’une électrode d’être fixées et interconnectées entre elles et entre le matériau actif de l’électrode et un collecteur, et l’électrode et un séparateur en contact avec ladite électrode sont liés l’un à l’autre par le biais d’une fusion à chaud. L’invention concerne également ledit lieur, qui a d’excellentes caractéristiques d’adhésion et de liaison thermique, et qui est donc utile pour un dispositif électrochimique comprenant des piles électrochimiques empilées et peut améliorer la qualité globale d’une batterie.
PCT/KR2006/001838 2005-05-17 2006-05-17 Lieur de polymere destine a un dispositif electrochimique comprenant plusieurs piles electrochimiques empilees WO2006123892A1 (fr)

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KR100515572B1 (ko) 2000-02-08 2005-09-20 주식회사 엘지화학 중첩 전기화학 셀 및 그의 제조 방법
KR100515571B1 (ko) 2000-02-08 2005-09-20 주식회사 엘지화학 중첩 전기 화학 셀
JP2001283853A (ja) 2000-03-30 2001-10-12 Nippon Zeon Co Ltd アルカリ二次電池負極用バインダー組成物およびその利用
US6656633B2 (en) * 2000-07-26 2003-12-02 Zeon Corporation Binder for electrode for lithium ion secondary battery, and utilization thereof
KR100644063B1 (ko) * 2003-06-03 2006-11-10 주식회사 엘지화학 분산제가 화학결합된 전극용 복합 바인더 중합체

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US20060275661A1 (en) 2006-12-07
KR20060119797A (ko) 2006-11-24
WO2006123892A1 (fr) 2006-11-23
CN100583514C (zh) 2010-01-20
KR100729118B1 (ko) 2007-06-14
JP5110599B2 (ja) 2012-12-26
US7935442B2 (en) 2011-05-03
JP2008546135A (ja) 2008-12-18

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